Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 23, Pages 7682-7686Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201901981
Keywords
bioelectrocatalysis; carbon dioxide fixation; formate dehydrogenase stabilization; mesoporous material
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Funding
- Center for Light Energy Activated Redox Processes (LEAP), an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0001059]
- Ryan Fellowship program of the Northwestern University International Institute of Nanotechnology
- Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource [NSF NNCI-1542205]
- MRSEC program at the Materials Research Center [NSF DMR-1720139]
- International Institute for Nanotechnology (IIN)
- Keck Foundation
- State of Illinois, through the IIN
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The efficient fixation of excess CO2 from the atmosphere to yield value-added chemicals remains crucial in response to the increasing levels of carbon emission. Coupling enzymatic reactions with electrochemical regeneration of cofactors is a promising technique for fixing CO2, while producing biomass which can be further transformed into biofuels. Herein, a bioelectrocatalytic system was established by depositing crystallites of a mesoporous metal-organic framework (MOF), termed NU-1006, containing formate dehydrogenase, on a fluorine-doped tin oxide glass electrode modified with Cp*Rh(2,2 '-bipyridyl-5,5 '-dicarboxylic acid)Cl-2 complex. This system converts CO2 into formic acid at a rate of 79 +/- 3.4mmh(-1) with electrochemical regeneration of the nicotinamide adenine dinucleotide cofactor. The MOF-enzyme composite exhibited significantly higher catalyst stability when subjected to non-native conditions compared to the free enzyme, doubling the formic acid yield.
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